Spectroscopic Identification of Active Sites of Oxygen-Doped Carbon for Selective Oxygen Reduction to Hydrogen Peroxide

Liu, L., Kang, L., Chutia, A. , Feng, J., Michalska, M., Ferrer, P., Grinter, D., Held, G., Tan, Y., Zhao, F., Guo, F., Hopkinson, D., Allen, C., Hou, Y., Gu, J., Papakonstantinou, I., Shearing, P., Brett, D., Parkin, I. and He, G. (2023) Spectroscopic Identification of Active Sites of Oxygen-Doped Carbon for Selective Oxygen Reduction to Hydrogen Peroxide. Angewandte Chemie, 135 (21). ISSN 1433-7851

Full content URL: https://doi.org/10.1002/ange.202303525

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Spectroscopic Identification of Active Sites of Oxygen-Doped Carbon for Selective Oxygen Reduction to Hydrogen Peroxide
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Abstract

The electrochemical synthesis of hydrogen peroxide (H2O2) via a two-electron (2e-) oxygen reduction reaction (ORR) process provides a promising alternative to replace the energy- intensive anthraquinone process. Herein, we develop a facile template-protected strategy to synthesize a highly active quinone- rich porous carbon catalyst for H2O2 electrochemical production. The optimized PCC900 material exhibits remarkable activity and selectivity, of which the onset potential reaches 0.83 V vs. reversible hydrogen electrode in 0.1 M KOH and the H2O2 selectivity is over 95 % in a wide potential range. Comprehensive synchrotron-based near-edge X-ray absorption fine structure (NEXAFS) spectroscopy combined with electrocatalytic characterizations reveals the positive correlation between quinone content and 2e- ORR performance. The effectiveness of chair-form quinone groups as the most efficient active sites is highlighted by the molecule-mimic strategy and theoretical analysis

Keywords:H2O2 electrochemical production, DFT
Subjects:F Physical Sciences > F100 Chemistry
Divisions:College of Science
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ID Code:53864
Deposited On:27 Apr 2023 10:50

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